Collaborative Research: Novel Materials and Reactor Design for Coupled Electrolytic Hydrogen Production and Nitrate Removal With Resource Recovery from Drinking Water

合作研究：耦合电解制氢和去除硝酸盐以及饮用水资源回收的新型材料和反应器设计

• 批准号: 1706797
• 负责人: Charles Werth
• 金额: $ 22.38万
• 依托单位: University of Texas at Austin
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-08-01 至 2020-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1706797&HistoricalAwards=false
• 关键词: Collaborative; Research; Novel; Materials; Reactor

1706797 / 1705255PIs : Werth, Charles J. / Jawahar Hussaini, Syed Mubeen Nitrate is the world's most ubiquitous groundwater pollutant, and its management is recognized as one of the Grand Challenges by the National Academy of Engineering. Catalytic treatment has emerged as a more sustainable option for nitrate removal from drinking water, but its implementation has been stymied by a lack of scientific knowledge and innovation in new materials that directly address challenges in reactor performance and scale-up. Specifically, nitrate treatment in scalable reactors is limited by hydrogen delivery to reactive catalysts sites. The PIs propose a high risk/high reward approach that is based on generating adsorbed atomic hydrogen in situ via electroactive catalyst supports. The overriding hypothesis is that atomic hydrogen can be electrolytically generated at the same (or directly adjacent to) site where nitrate reduction occurs, and this generation can be balanced with nitrate reduction to eliminate hydrogen mass transfer limitations, optimize hydrogen use, minimize energy consumption, and recover value-added resources, ammonium and chlorine. The specific objectives of the proposed work are: 1) To identify the fundamental bulk material and surface chemical properties responsible for the synthesis of carbon-based catalyst supports with high-electrical conductivity, metal dispersion, water permeability, and strength. 2) To elucidate reaction mechanisms and kinetics of coupled electrolytic hydrogen generation and nitrate reduction processes in batch and flow-through reactors, and to identify the fundamental properties of new catalytic materials that optimize these processes. 3) To evaluate the economic and environmental sustainability of a hybrid ion exchange - electrochemical reactor for nitrate removal from drinking water.The proposed approach involves novel synthesis and electro/catalytic experiments that aim to elucidate structure/property correlations, reaction mechanisms, and optimal reactor conditions for efficient nitrate removal coupled with ammonia recovery from simulated drinking water, and an economic and environmental life cycle analyses of the technology coupled to ion exchange waste brine treatment and reuse that will serve as feedback for process optimization. Potential scientific advancements include: (i) foundational insights and structure-activity relationships to guide synthesis of new cathodic materials that efficiently generate hydrogen and reduce nitrate at catalytically reactive sites; (ii) the design of a novel electrolytic- based reactor that integrates these robust cathodic materials into a packed-bed flow system; (iii) integrated resource recovery of agriculturally valuable ammonium, as well as chlorine for catalyst fouling mitigation and water disinfection; and (iv) the development and dissemination of an integrated model that allows scale up for a cost and environmental impact assessment for new technology development. Proposed educational, outreach and engagement activities include using UT Austin's engineering open houses to expose junior high and high school students to engineering design for water treatment the development of a new teaching modules and dissemination to water utilities through an industry collaborator.

硝酸盐是世界上最普遍存在的地下水污染物，其管理被美国国家工程院认定为重大挑战之一。催化处理已经成为饮用水中硝酸盐去除的一种更可持续的选择，但由于缺乏科学知识和新材料的创新，它的实施一直受到阻碍，这些新材料无法直接解决反应器性能和规模方面的挑战。具体来说，可伸缩反应器中的硝酸盐处理受到氢输送到活性催化剂位点的限制。PIs提出了一种高风险/高回报的方法，该方法基于通过电活性催化剂载体在原位产生吸附的原子氢。最重要的假设是，原子氢可以在发生硝酸盐还原的相同（或直接邻近）位置电解生成，并且可以与硝酸盐还原平衡，以消除氢的传质限制，优化氢的利用，最小化能耗，并回收增值资源，铵和氯。该工作的具体目标是：1)确定合成具有高导电性、金属分散性、透水性和强度的碳基催化剂载体的基本大块材料和表面化学性质。2)阐明间歇式反应器和流式反应器中电解制氢和硝酸还原耦合过程的反应机理和动力学，并确定优化这些过程的新型催化材料的基本性质。3)评价离子交换-电化学混合反应器去除饮用水中硝酸盐的经济和环境可持续性。提出的方法包括新的合成和电/催化实验，旨在阐明结构/性质相关性，反应机制，以及有效去除硝酸盐和从模拟饮用水中回收氨的最佳反应器条件，并对该技术进行经济和环境生命周期分析，结合离子交换废盐水处理和再利用，将作为过程优化的反馈。潜在的科学进展包括：(i)基础见解和结构-活性关系，指导合成新的阴极材料，有效地产生氢和减少催化反应部位的硝酸盐；（ii）设计一种新型电解反应器，将这些坚固的阴极材料集成到填充床流系统中；（三）综合资源回收农业上有价值的铵，以及用于减轻催化剂污染和水消毒的氯；（四）发展和传播一种综合模式，以便扩大对新技术发展的成本和环境影响评估的规模。拟议的教育、推广和参与活动包括利用德克萨斯大学奥斯汀分校的工程开放日，向初中和高中学生展示水处理的工程设计，开发新的教学模块，并通过行业合作伙伴向水务公司传播。

项目成果

Scalable Reactor Design for Electrocatalytic Nitrite Reduction with Minimal Mass Transfer Limitations

• DOI: 10.1021/acsestengg.0c00054
• 发表时间: 2020-11
• 作者: Chenxu Yan;Sruthi Kakuturu;Ashley Hesterberg Butzlaff;David M. Cwiertny;Syed Mubeen;C. Werth

Electrospun TiO 2 /carbon composite nanofibers as effective (photo)electrodes for removal and transformation of recalcitrant water contaminants

电纺 TiO 2 /碳复合纳米纤维作为有效（光）电极去除和转化顽固水污染物

• DOI: 10.1039/d3va00017f
• 发表时间: 2023
• 期刊: Environmental Science: Advances
• 作者: Butzlaff, Ashley Hesterberg;Jensen, Madeline;Yan, Chenxu;Ghanim, Abdulsattar;Werth, Charles;Cwiertny, David;Mubeen, Syed
• 通讯作者: Mubeen, Syed

Factors Impeding Replacement of Ion Exchange with (Electro)Catalytic Treatment for Nitrate Removal from Drinking Water

• DOI: 10.1021/acsestengg.0c00076
• 发表时间: 2020-10
• 期刊: ACS ES&T Engineering
• 影响因子: 7.1
• 作者: C. Werth;Chenxu Yan;Jacob P. Troutman